Coupled in-situ H2O2 generation and utilization over donor-acceptor covalent organic frameworks for rapid photocatalytic U(VI) removal

Uranium-contaminated water streams associated with nuclear fuel cycle operations represent an emerging challenge in water purification, combining radiological risk with the opportunity for resource recovery. Developing sustainable uranium removal technologies that operate under mild conditions while minimizing chemical inputs remains a critical task, particularly for integration into advanced water treatment systems. Herein, we report a donor-acceptor covalent organic framework (DANT-TFPT) featuring an in-framework coupled H 2 O 2 production and consumption (IFC-HPC) architecture for photocatalytic uranium removal. By co-localizing oxygen reduction reaction catalytic sites and uranyl-binding pockets within a single scaffold, photogenerated H 2 O 2 is produced and consumed in-situ, minimizing diffusion losses and nonproductive decomposition. Together with strong donor-acceptor coupling and abundant N/O-rich coordination domains, the DANT-TFPT exhibits a high H 2 O 2 evolution rate under ambient air to achieve an exceptional U(VI) uptake capacity of 745.7 mg g −1 with a fast removal rate of 67.8 mg g −1  h −1 without sacrificial reagents in uranium-contaminated wastewater. This study demonstrates a chemical-efficient and environmentally benign strategy for the removal and recovery of uranium from contaminated waters, highlighting the potential of integrated photocatalytic-sorptive materials for emerging contaminant control and resource recovery in water purification and desalination-related treatment processes.